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The first building for the Ursuline nuns in New Orleans was designed by Ignace François Broutin in 1727 when the nuns arrived in New Orleans. Michael Zeringue (Johann Michael Zehringer), the King's Master Carpenter from Franconia, Bavaria and progenitor of all "Zeringue" families in Louisiana was the builder. Planning, collecting material, and construction took years. Existing drawings show the building in 1733, although it was not officially finished until the following year.

Colombage (half-timbered) or briquette-entre-poteaux (brick-between-post) was the major form of French Colonial construction in the colony during the 18th century (see also Pitot House). Usually the exterior walls were then given a protective covering of stucco or wooden boards; but the fact that the timbered walls of the Ursuline Convent were left exposed is confirmed by a drawing from 1737. Such construction proved to be inappropriate for the humid climate of New Orleans (with significant deterioration already apparent by 1745),[1] in addition to being a fire hazard.

In 1745 plans for a new building of brick and protected colombage were prepared by Ignace Broutin. The contractor was Claude Joseph Villars Dubreuil, Contractor of Public Works for the King. His wife, Marie Payen de Noyan, was Bienville's sister. This structure was completed in 1751. It is likely that Alexandre de Batz also took part in the design because several payments are listed to him for work on the new building. The new building was laid out adjacent to the site of the older structure, and some materials from the older building were used in the construction of the newer one.

Built of stucco-covered brick, the new building, also known as Old Ursuline Convent, is typical for the French neoclassical architecture. It is a formal, symmetrical building, severely designed in its lack of ornamentation. No applied orders of pilasters or columns relieved the plain walls. Only the slightly arched window set in shallow moldings, the rusticated quoins at the corners and narrow central pedimented pavilion break the even rhythm of the fenestration. The broad plain hipped roof, broken only by small low-set dormers contrasts well with the multi-windowed façade and completes the austere but not unpleasant, finely proportioned building.

The ground floor was used largely for the dormitory, classrooms, refectory, and infirmary of the orphanage, maintained by the nuns.[1] The second floor contained cells for the nuns, a library, (another) infirmary, and storerooms. The winding stairway visible from the main entrance hallway is believed to be from the original convent, installed in the new building.

"This is the finest surviving example of French colonial public architecture in the country," states the National Park Service.[3] It is by some accounts the oldest structure in New Orleans, built between 1748 and 1752.

The convent and its associated school, Ursuline Academy, moved downriver to a site on Dauphine Street in the 9th Ward in 1824, turning over the original convent to the Bishop of New Orleans. It was then referred to as the “Archbishop’s Palace".[1] In 1912 the convent moved uptown to State Street.

The entrance portico was added by the Bishop, who also constructed the gatehouse around 1825-1830 and reoriented the building, which originally faced the river, to have the main entrance on what had been the back side (Chartres Street). The Ursuline property covered two city squares, extending to Royal Street. An old ground plan shows a chapel at the corner of Ursulines and Decatur Streets, dedicated to Our Lady of Victory. Near the entrance to the grounds, along the levee, were also a reception house for visitors, the day school, and a residence for the chaplain. Between these buildings and the convent were gardens. To the right, moving up from the riverside entrance, were the hospital buildings, and beyond them military barracks.

Despite great interior alterations and decay, the Convent is considered one of the most important historical and religious landmarks in the United States and is one of the few remaining physical links with the French colonial period in Louisiana.

In 1824 the nuns moved to a new larger convent in the city's 9th Ward, and the present structure was turned over to the Bishop of New Orleans as a residence, and for a while came to be called "the Archbishop's Palace". After 1899 it continued in use as offices for the Archdiocese and still later as a rectory for the adjacent St. Mary's Church.